Beijing Key Laboratory for Green Catalysis and Separation, Key Laboratory of Beijing on Regional Air Pollution Control, Key Laboratory of Advanced Functional Materials, Education Ministry of China, Laboratory of Catalysis Chemistry and Nanoscience, Department of Chemistry and Chemical Engineering, College of Environmental and Energy Engineering , Beijing University of Technology , Beijing 100124 , P. R. China.
Environ Sci Technol. 2019 May 21;53(10):5926-5935. doi: 10.1021/acs.est.9b00370. Epub 2019 May 9.
Since the conventional Pd-based catalysts often suffer severe deactivation by water, development of a catalyst with good activity and moisture-resistance ability is of importance in effectively controlling emissions of volatile organic compounds (VOCs). Herein, we report the efficient synthesis of ultrathin palladium-tungsten bimetallic nanosheets with exceptionally high dispersion of tungsten species. The supported catalyst (TiO/PdW) shows good performance for benzene oxidation, and 90% conversion is achieved at a temperature of 200 °C and a space velocity of 40 000 mL g h. The TiO/PdW catalyst also exhibits better water-tolerant ability than the traditional Pd/TiO catalyst. The high catalytic efficiency can be explained by the facile redox cycle of the active Pd/Pd couple in the close-contact PdO -WO -TiO arrangement. We propose that the reason for good tolerance to water is that the lattice oxygen of the TiO/PdW catalyst can effectively replenish the oxygen in active PdO sites consumed by benzene oxidation. A four-step benzene transformation mechanism promoted by the catalyst is proposed. The present work provides a useful idea for the rational design of efficient bimetallic catalysts for the removal of VOCs under the high humidity conditions.
由于传统的钯基催化剂通常会因水而严重失活,因此开发一种具有良好活性和耐湿性的催化剂对于有效控制挥发性有机化合物(VOC)的排放非常重要。在此,我们报告了具有高分散钨物种的超薄钯-钨双金属纳米片的高效合成。负载型催化剂(TiO/PdW)在苯氧化中表现出良好的性能,在 200°C 的温度和 40 000 mL g h 的空速下可实现 90%的转化率。与传统的 Pd/TiO 催化剂相比,TiO/PdW 催化剂还表现出更好的耐水性。高催化效率可以通过在紧密接触的 PdO-WO-TiO 排列中活性 Pd/Pd 对的易还原氧化循环来解释。我们提出,对水具有良好耐受性的原因是 TiO/PdW 催化剂的晶格氧可以有效地补充苯氧化消耗的活性 PdO 位中的氧。提出了一种由催化剂促进的四步苯转化机理。本工作为在高湿度条件下去除 VOC 提供了一种设计高效双金属催化剂的有用思路。